The datatable is the data source for your grid view. So, if you want to add items to the view, you have to add them to its data source.
You should use
DataTable.NewRow Method[
^] instead.
Not knowing the schema of the datatable, it is hard to provide a more concrete answer, but the link holds an example of method's usage, and you can start with it and see where it gets you.
Hope this helps.